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Register a new userDesigner Magnetism in High Entropy Oxides
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Thomas Zac Ward PhD
Publication date
2021
fields
Physics
and research's language is
English
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Disorder can have a dominating influence on correlated and quantum materials leading to novel behaviors which have no clean limit counterparts. In magnetic systems, spin and exchange disorder can provide access to quantum criticality, frustration, and spin dynamics, but broad tunability of these responses and a deeper understanding of strong limit disorder is lacking. In this work, we demonstrate that high entropy oxides present an unexplored route to designing quantum materials in which the presence of strong local compositional disorder hosted on a positionally ordered lattice can be used to generate highly tunable emergent magnetic behavior--from macroscopically ordered states to frustration-driven dynamic spin interactions. Single crystal La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 films are used as a structurally uniform model system hosting a magnetic sublattice with massive microstate disorder in the form of site-to-site spin and exchange type inhomogeneity. A classical Heisenberg model is found to be sufficient to describe how compositionally disordered systems can paradoxically host long-range magnetic uniformity and demonstrates that balancing the populating elements based on their discrete quantum parameters can be used to give continuous control over ordering types and critical temperatures. Theory-guided experiments show that composite exchange values derived from the complex mix of microstate interactions can be used to design the required compositional parameters for a desired response. These predicted materials are synthesized and found to possess an incipient quantum critical point when magnetic ordering types are designed to be in direct competition; this leads to highly controllable exchange bias sensitivity in the monolithic single crystal films previously accessible only in intentionally designed bilayer heterojunctions.
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The possibility of investigating the dynamics of solids on timescales faster than the thermalization of the internal degrees of freedom has disclosed novel non-equilibrium phenomena that have no counterpart at equilibrium. Transition metal oxides (TMOs) provide an interesting playground in which the correlations among the charges in the metal $d$-orbitals give rise to a wealth of intriguing electronic and thermodynamic properties involving the spin, charge, lattice and orbital orders. Furthermore, the physical properties of TMOs can be engineered at the atomic level, thus providing the platform to investigate the transport phenomena on timescales of the order of the intrinsic decoherence time of the charge excitations. Here, we review and discuss three paradigmatic examples of transient emerging properties that are expected to open new fields of research: i) the creation of non-thermal magnetic states in spin-orbit Mott insulators; ii) the possible exploitation of quantum paths for the transport and collection of charge excitations in TMO-based few-monolayers devices; iii) the transient wave-like behavior of the temperature field in strongly anisotropic TMOs.
We investigate spin correlations in the dipolar Heisenberg antiferromagnet Gd2Sn2O7 using polarised neutron-scattering measurements in the correlated paramagnetic regime. Using Monte Carlo methods, we show that our data are sensitive to weak further-neighbour exchange interactions of magnitude ~0.5% of the nearest-neighbour interaction, and are compatible with either antiferromagnetic next-nearest neighbour interactions, or ferromagnetic third-neighbour interactions that connect spins across hexagonal loops. Calculations of the magnetic scattering intensity reveal rods of diffuse scattering along [111] reciprocal-space directions, which we explain in terms of strong antiferromagnetic correlations parallel to the set of <110> directions that connect a given spin with its nearest neighbours. Finally, we demonstrate that the spin correlations in Gd2Sn2O7 are highly anisotropic, and correlations parallel to third-neighbour separations are particularly sensitive to critical fluctuations associated with incipient long-range order.
The 18.5 K superconductor PuCoGa5 has many unusual properties, including those due to damage induced by self-irradiation. The superconducting transition temperature decreases sharply with time, suggesting a radiation-induced Frenkel defect concentration much larger than predicted by current radiation damage theories. Extended x-ray absorption fine-structure measurements demonstrate that while the local crystal structure in fresh material is well ordered, aged material is disordered much more strongly than expected from simple defects, consistent with strong disorder throughout the damage cascade region. These data highlight the potential impact of local lattice distortions relative to defects on the properties of irradiated materials and underscore the need for more atomic-resolution structural comparisons between radiation damage experiments and theory.
The interplay of symmetry and quenched disorder leads to some of the most fundamentally interesting and technologically important properties of correlated materials. It also poses the most vexing of theoretical challenges. Nowhere is this more apparent than in the study of spin glasses. A spin glass is characterized by an ergodic landscape of states - an innumerable number of possibilities that are only weakly distinguished energetically, if at all. We show in the material Fe$_x$NbS$_2$, this landscape of states can be biased by coexisitng antiferromagnetic order. This process leads to a phenomenon of broad technological importance: giant, tunable exchange bias. We observe exchange biases that exceed those of conventional materials by more than two orders of magnitude. This work illustrates a novel route to giant exchange bias by leveraging the interplay of frustration and disorder in exotic materials.
We study the quantum criticality of the phase transition between the Dirac semimetal and the excitonic insulator in two dimensions. Even though the system has a semimetallic ground state, there are observable effects of excitonic pairing at finite temperatures and/or finite energies, provided that the system is in proximity to the excitonic insulating transition. To determine the quantum critical behavior, we consider three potentially important interactions, including the Yukawa coupling between Dirac fermions and the excitonic order parameter fluctuation, the long-range Coulomb interaction, and the disorder scattering. We employ the renormalization group technique to study how these interactions affect quantum criticality and also how they influence each other. We first investigate the Yukawa coupling in the clean limit, and show that it gives rise to typical non-Fermi liquid behavior. Adding random scalar potential to the system always turns such a non-Fermi liquid into a compressible diffusive metal. In comparison, the non-Fermi liquid behavior is further enhanced by random vector potential, but is nearly unaffected by random mass. Incorporating the Coulomb interaction may change the results qualitatively. In particular, the non-Fermi liquid state is protected by the Coulomb interaction for weak random scalar potential, and it becomes a diffusive metal only when random scalar potential becomes sufficiently strong. When random vector potential or random mass coexists with Yukawa coupling and Coulomb interaction, the system is a stable non-Fermi liquid state, with fermion velocities flowing to constants in the former case and being singularly renormalized in the latter case. These quantum critical phenomena can be probed by measuring observable quantities.
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